Reactor for synthesis of methanol or other products

ABSTRACT

An improved reactor comprising a shell and at least one reactor internal component. The reactor internal component includes a tube bundle comprising a plurality of tubes attached by at least one tube support plate comprising at least one radial strut and at least one bracket configured to secure to at least one tube of the tube bundle. The tubes are arranged in concentric bands about a longitudinal axis of the reactor. The reactor can also include a gas inlet plate, a catalyst support plate, and a top plate. The reactor shell can include a domed head portion with a startup nozzle connected to a reducing flange, providing a manhole access opening into the shell. Sliding strips that slide relative to the tube support plates can facilitate easier assembly, and support rings for the tubes adjacent the plates can accommodate variable thermal expansion of the tubes received in the plates.

CROSS REFERENCE TO RELATED APPLICATION(S)

This application is a continuation-in-part under 35 U.S.C 120 of U.S.application Ser. No. 17/574,992, filed Jan. 13, 2022, which claims thebenefit of priority under 35 U.S.C 119(e) to U.S. ProvisionalApplication No. 63/138,022, filed Jan. 15, 2021. The entire contents ofeach of the foregoing applications is incorporated herein by reference.

FIELD OF THE DISCLOSURE

The disclosure relates to a reactor, in particular to a reactor formethanol synthesis.

BACKGROUND

Global climate change has been deemed to be the “most pressingenvironmental challenge of our time.” The National Aeronautics and SpaceAdministration (NASA) cites that “scientific evidence for warming of theclimate system is unequivocal.” Climate change results from the warmingeffects of greenhouse gases such as water vapor, nitrous oxide, methane,and carbon dioxide. Of these, carbon dioxide emissions are a keyculprit, as global atmospheric concentration of CO₂ has increased by athird since the Industrial Revolution began. CO₂ emissions largely stemfrom human activities, such as the consumption of fossil fuels, thebyproducts of which are emitted into the atmosphere.

Chemical energy storage has been explored as a solution to the problemof renewable energy sources such as wind and solar power beinginherently intermittent and unpredictable. Because of the intermittencyof wind and solar power, power grids and utilities must meet baselinepower demands through fossil fuel-based sources, with suddenly availablewind and solar power being difficult to incorporate into the grid due tothe difficulty of quickly scaling down and scaling up such fossilfuel-based sources, like coal-fired power plants. Because many renewableenergy sources are difficult to scale up as a replacement fortraditional fossil fuel-based power sources, high-density energy storageof renewable energy, such that the renewable energy can be stored andused when the grid is able to accommodate the energy, is critical forcombating climate change.

Existing energy storage modalities, including thermal energy storage,compressed air energy storage, hydrogen storage, pumped hydroelectricstorage, and large-scale batteries have so far proven to beprohibitively expensive and/or difficult to scale up. Chemical storageof renewable energy in the form of electrolyzing water to producehydrogen, such as for combustion, fuel cell consumption, or chemicalsynthesis such as methanol synthesis, is a promising approach toproviding sufficiently dense and stable storage of renewable energy thatmay be used when needed, allowing renewable energy to supply energyneeds consistently rather than intermittently.

Reactors used in methanol synthesis from syngas are typically limited toboiling water reactors (BWRs) due to the high heat profile of typicalreaction suites, which include substantial amounts of CO. BWRs arecomplex and expensive equipment, but are typically necessary in order tomitigate the heat generated from the exothermic production of methanolfrom syngas in order to protect the reaction product, the reactor, andthe catalyst.

Shell-and-tube reactors for catalytic and/or exothermic reactions, suchas synthesizing methanol from CO₂ and H₂ using a suitable catalyst suchas a copper and zinc oxide (Cu/ZnO)-based catalyst or other suitablecatalyst, must receive regular maintenance, such as loading and/orremoving and recharging catalyst, de-fouling the reactor shell,performing repairs of various components, or otherwise. The ability toaccess the interior of the reactor for loading catalyst, performingmaintenance, and other purposes must be balanced against the need toretain the tubes in a bundle.

Existing designs of shell-and-tube reactors are difficult to scale up orscale down based on the needs of a particular facility, such as adesired throughput. The throughput of the facility may change with timedue to debottlenecking efforts, which may increase the throughputrequirements of the reactor. Scaling up a reactor for debottlenecking afacility can be a difficult, expensive, and time-consuming endeavor,with the entire reactor, including the internals, needing to be revampedor redesigned in many instances.

This can require significant design and engineering effort, as anengineer must essentially “reinvent the wheel” when scaling up thedesign, with consideration given to the arrangement and cross-sectionalarea of the tubes, the size and configuration of the shell, the volumeand cross-sectional surface area of the catalyst bed, among otherthings. Existing shell-and-tube reactor designs and providers are poorlysuited to adapting reactor designs to changing requirements in anefficient manner. If the reactor is not properly designed, unevendistribution of catalyst, reactants, and heat may result, which candamage the catalyst and/or components of the reactor and reduce theefficiency of the reaction. In some cases, a runaway exothermic reactioncan result in catastrophic failure of the reactor.

Additionally, it is difficult to scale and properly fabricate feed tubesin and/or for a reactor. Improperly designed, arranged, and/orfabricated feed tubes often lead to the creation of blockages, eddies,and uneven areas of reactants within reactors, which disadvantageouslyreduces the efficiency and throughput of a reactor and can result in hotspots. Hot spots in exothermic reactions are particularly dangerous anddamaging to the reactor and catalyst.

Another problem in reactor design is the difficulty of measuringinternal reactor temperature at one or more desired locations. It isdifficult to properly control a process including a reactor,particularly in high-risk applications such as exothermic reactions,without an understanding of the temperature profile of the reactorinternals, particularly at different locations along the reactor bodycorresponding to different stages of the reaction and/or differentreactor conditions.

However, thermocouple joints including a gasket seat may sustain damageover time, leading to thermocouple joint leakage. While such leakagesmay be repaired, doing so requires deactivating the catalyst andreplacing the gasket seat. This involves costly, potentially dangerous,and time-consuming shut-downs, deactivation of catalyst, and start-ups,each of which entails high costs, including substantial opportunitycosts. Given that the expected lifetime of catalysts tends to be betweenthree and five years, such repairs constitute highly expensivedisruptions to the operation of a facility. Further, in high pressureand/or temperature reactions involving hydrogen, the risk of leakagefrom flanged joints is particularly high, both of hydrogen or otherreactants/products outwardly and of oxygen, a catalyst poison, inwardly.

Accordingly, existing reactor designs that incorporate multiplethermowells for providing thermocouples at different elevationallocations along a reactor body are susceptible to significantoperational disruptions due to thermocouple joint leakage, and reactordesigns that omit such thermowells to avoid disruptions lack thenecessary reactor-conditions data to properly control the reaction.Additionally, existing thermowell configurations in reactors insert thethermocouple transversely to a flow direction, e.g. radially into thereactor body. This disadvantageously results in temperature readings forlarger reactors of conditions close to the outer shell, which furtherrenders scaling of a reactor design difficult. Reactor designs arefurther ill-suited to allowing a thermocouple to be inserted into thereactor body when the catalyst is present without damaging thethermocouple.

Existing reactor designs may comprise one or more nozzles for unloadingspent catalyst, for example from a bottom portion of the reactor body.The configuration of existing reactors' catalyst-unloading nozzles ispoorly adapted to effectively and quickly removing catalyst, such thatan operator must scrape catalyst out of the reactor body.

Certain shell-and-tube-type reactors and other types of reactors maycomprise an inlet nozzle from which reactant gases are routed through apipe extending through a center of the reactor body. The pipe may bedrilled to fit one or more feed tubes, which each may be bent to bothconnect to the pipe and then feed the reactant upwardly through thereactor body. Such reactor configurations are not adapted to scaling up,for example to several hundred tubes, given the precise andtube-specific adjustments that must be made to connect the pipe to eachof the feed tubes.

The inlet pipe in certain reactor configurations is further utilized tosupport the feed tubes at different elevations within the reactor body,with one or more flat bars welded to and extending between the inletpipe and one or more feed tubes. This configuration is highlytime-consuming particularly for manufacturing, assembling, andmaintaining a large-scale reactor, which complicates the task of scalinga reactor design depending on the requirements of a facility.Additionally, the inlet pipe disadvantageously occupies significantcross-sectional area that could otherwise be occupied by catalyst. Whiletie rods have been contemplated for supporting feed tubes inshell-and-tube reactors, such supports take up catalyst space andpresent obstructions during catalyst loading and unloading.

From the foregoing, there is a need for an improved reactor that isconfigured for maintaining the reactor internals and managing thecatalyst, for scaling the reactor throughput up or down based on thethroughput needs of a facility, for improved measurement of reactorconditions without compromising reactor integrity and maintainability,for effectively removing spent catalyst, for improved manufacture, andfor overcoming the challenges of constructing a shell-and-tube reactor.

SUMMARY

Reactor embodiments according to the present disclosure advantageouslyaddress the drawbacks of existing reactor designs by providing a reactorthat is scalable and/or configured for improved access andmaintainability of the reactor, particularly of an interior of thereactor. The reactor embodiments may be configured to facilitate accessto the reactor internals without sacrificing strength and robustness ofthe reactor internals, such as a reactor tube bundle comprising one ormore tubes and one or more support structures, such that the tube bundleremains intact and undamaged.

The reactor embodiments further comprise a tube arrangement that isconfigured for scaling up or down readily based on the needs of aparticular facility. Whereas in existing reactor designs, tubes cannotbe easily added to or removed from a tube bundle in accordance with areactor shell shape when building a reactor without significant redesignwork, the embodiments of the present disclosure advantageously allow forcircumferential bands or other arrangements of tubes to be modularlyarranged based on the required throughput of the reactor and theassociated facility. In embodiments the arrangements of tubes may defineregular and/or repeating patterns that can be simply added to and/orremoved from an existing tube bundle design when designing a reactor.This has the advantage of making debottlenecking operations or otherdesign work much easier and less costly from a manufacturingperspective.

The arrangement of the tube bundle further facilitates heat and reactantdistribution throughout the reactor interior, in particular through thecatalyst bed, without disrupting catalyst loading, which typicallyoccurs as an operator loads or dumps the catalyst particles into thereactor interior from an open top end of the reactor. The arrangement ofthe reactor and the tube bundle of embodiments advantageously providesboth modularity of design for improved constructability whilemaintaining desired properties regarding heat and reactant distributionwhile also ensuring that the catalyst particles are evenly distributedwithin the reactor interior.

The tube bundle of reactor embodiments according to the disclosure arefurther configured to provide improved structural support to one or moretubes for increased robustness of the reactor during construction,transportation, and installation, as well as during operation. Inembodiments, one or more structural supports are provided and/or one ormore of the tubes is provided with increased thickness for ensuringstructural support at desired locations of the tube bundle.

In embodiments, the reactor and components thereof are configured tofacilitate easy access for maintenance of critical parts. One or moreplates configured for supporting the tube bundle may be modular suchthat an operator may load catalyst, unload catalyst, or accesscomponents in the reactor interior with ease compared to existingreactors, where components such as support plates are welded to aninterior surface of the reactor shell and prohibit access to the reactorinternal components.

The reactor embodiments address the problem of existing reactor designsbeing poorly suited to provide proper flow and reactant distribution,and consequently heat distribution, within the reactor and the catalystbed, by providing an improved inlet nozzle and distribution mechanismconfigured to directing reactants into a tube bundle arranged within aninterior of the reactor. in embodiments, the inlet nozzle is providedproximate a gas inlet plate and is arranged with a flow directiontransverse to a flow direction of the tubes of the tube bundle. Asecondary inlet nozzle may be provided at a bottom of the reactor andmay be configured with a structure for evenly distributing flow into thetubes of the tube bundle. In embodiments, one or more catalyst unloadingnozzles are provided in an improved configuration for removing catalyst,with the unloading nozzles configured at a downward angle.

The tube bundle and the tubes may be arranged such that across-sectional area of the tubes relative to a cross-sectional area ofthe catalyst is improved for even heat and flow distribution withoutinterfering with the structural and modularity features of the tubebundle.

The reactor embodiments are further configured to reduce the incidenceof blockages, eddies, and/or uneven areas of reactants within thereactor body and accompanying hot spots by providing for an improveddistribution of catalyst, reactor internals, and reactants during thecourse of a reaction.

The reactor embodiments of the present disclosure further address thedisadvantages of existing reactor designs regarding process control andtemperature measurement. In embodiments, the reactor is configured toprovide one or more thermowells configured to receive one or morerespective thermocouples. The thermocouples may be configured to measurea temperature of the reactor interior at a plurality of locations usingrespectively a single thermowell arranged axially or longitudinallyrelative to the reactor body.

An example embodiment according to the present disclosure may bedirected to a reactor, comprising: a shell defining an internal space;at least one inlet nozzle; and a tube bundle comprising one or moretubes.

An embodiment may further comprise a catalyst support plate.

An embodiment may further comprise at least one tube support plate.

An embodiment may further comprise a gas inlet plate.

An embodiment may further comprise a top plate.

An embodiment may further comprise a top plate and tube support plate.

An embodiment may further be configured where the shell is configured toreceive at least one catalyst.

In an embodiment, the at least one catalyst is a solid catalyst. Suchcatalyst may comprise balls of a first diameter.

In an embodiment the solid catalyst comprises balls of a seconddiameter.

In embodiment the shell is configured to receive at least one solidcatalyst. Such solid catalyst may comprise a shape defining at least oneof pellets, rings, tablets, or spheres.

In an embodiment, the catalyst support plate is configured to support aheight of the solid catalyst.

In an embodiment, the catalyst support plate defines one or moreapertures.

In an embodiment, the one or more apertures comprise a plurality ofapertures of a first size and a plurality of apertures of a second size,the apertures extending through at least part of a thickness of thecatalyst support plate.

In an embodiment, the first size corresponds to a circumference of atleast one tube of the tube bundle.

In an embodiment, the second size is smaller than the first size.

In an embodiment, the second size is a function of the thickness of thecatalyst support plate.

In an embodiment, the apertures of the first size are defined throughthe catalyst support plate according to an arrangement of the pluralityof tubes.

In an embodiment, the gas inlet plate comprises a plurality of aperturesdefined through a thickness of the gas inlet plate.

In an embodiment, the plurality of apertures are circular aperturesdefined through the gas inlet plate according to the arrangement of theplurality of tubes.

In an embodiment, the gas inlet plate further comprises a secondplurality of apertures defined through the thickness of the gas inletplate, the second plurality of apertures comprising a different sizeand/or shape than the plurality of circular apertures.

In an embodiment, the shell defines an outlet nozzle.

In an embodiment, the outlet nozzle is located at a side portion of theshell.

In an embodiment, the inlet nozzle is located proximate a bottom portionof the shell.

In an embodiment, the inlet nozzle is arranged transverse to a directionof flow through the shell.

In an embodiment, the inlet nozzle is arranged substantially parallel toa direction of flow through the shell.

In an embodiment, the gas inlet plate is arranged proximate the inletnozzle.

In an embodiment, the at least one tube support plate comprises at leastone circumferential band.

In an embodiment, the at least one circumferential band comprises atleast one bracket configured to extend about a portion of a tube of thetube bundle.

In an embodiment, the at least one bracket extends about an entirety ofthe tube.

In an embodiment, the shell defines a startup nozzle configured for theprovision of a heating fluid.

In an embodiment, the reactor further comprises at least one catalystunloading nozzle.

In an embodiment, the reactor further comprises a hand hole.

In an embodiment, the at least one tube support plate defines aplurality of concentric circumferential bands.

In an embodiment, the tube bundle comprises at least one tube of a firstsize and at least one tube of a second size.

In an embodiment, the inlet nozzle is arranged below the gas inletplate.

In an embodiment, the shell defines an outlet nozzle, and wherein theoutlet nozzle is arranged below the catalyst support plate.

In an embodiment, catalyst (e.g., balls) of the first size (e.g.,diameter) and the catalyst (e.g., balls) of the second size (e.g.,diameter) are arranged in discrete, respective layers proximate thecatalyst support plate.

In an embodiment, the shell is configured to receive at least one solidcatalyst, wherein the catalyst defines a first height within the shellin an unreduced state and a second height within the shell in a reducedstate (e.g., due to settling that may occur during operation).

In an embodiment, the second height is lower than the first height.

In an embodiment, the at least one tube support plate defines at leastone radial strut connected to at least one of the plurality ofcircumferential bands.

In an embodiment, the at least one radial strut connects to at least oneof the circumferential bands and to an outer support band.

In an embodiment, an innermost circumferential band of the at least onetube support plate comprises a number of brackets (e.g., six) configuredrespectively to correspond to a ring of the same number of innermosttubes of a first size.

In an embodiment, a second circumferential band of the at least one tubesupport plate comprises an equal or greater number of brackets than theprevious band (e.g., 10) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the second concentric band or ring of tubes. Suchtubes may be of the first size.

In an embodiment, a third circumferential band of the at least one tubesupport plate comprises an equal or greater number of brackets than theprevious band (e.g., 14) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the third concentric band or ring of tubes. Such tubesmay be of the second size.

In an embodiment, a fourth circumferential band of the at least one tubesupport plate comprises an equal or greater number of brackets than theprevious band (e.g., 18) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the fourth concentric band or ring of tubes. Suchtubes may be of the first size.

In an embodiment, a fifth circumferential band of the at least one tubesupport plate comprises an equal or greater number of brackets than theprevious band (e.g., 22) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the fifth concentric band or ring of tubes. Such tubesmay be of the first size.

In an embodiment, a sixth circumferential band of the at least one tubesupport plate comprises an equal or greater number of brackets than theprevious band (e.g., 26) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the sixth concentric band or ring of tubes. Such tubesmay be of the first size.

In an embodiment, a seventh circumferential band of the at least onetube support plate comprises an equal or greater number of brackets thanthe previous band (e.g., 30) brackets configured respectively tocorrespond to a concentric band (e.g., ring) of the same number of tubesof the tube bundle located in the seventh concentric band or ring oftubes. Such tubes may be of the second size.

In an embodiment, an eighth circumferential band of the at least onetube support plate comprises an equal or greater number of brackets thanthe previous band (e.g., 34) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the eighth concentric band or ring of tubes. Suchtubes may be of the first size.

In an embodiment, a ninth circumferential band of the at least one tubesupport plate comprises an equal or greater number of brackets than theprevious band (e.g., 36) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the ninth concentric band or ring of tubes. Such tubesmay be of the first size.

In an embodiment, a tenth circumferential band of the at least one tubesupport plate comprises an equal or greater number of brackets than theprevious band (e.g., 42) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the tenth concentric band or ring of tubes. Such tubesmay be of the first size.

In an embodiment, an eleventh circumferential band of the at least onetube support plate comprises an equal or greater number of brackets thanthe previous band (e.g., 46) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the eleventh concentric band or ring of tubes. Suchtubes may be of the second size.

In an embodiment, a twelfth circumferential band of the at least onetube support plate comprises an equal or greater number of brackets thanthe previous band (e.g., 50) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the twelfth concentric band or ring of tubes. Suchtubes may be of the first size.

In an embodiment, a thirteenth circumferential band of the at least onetube support plate comprises an equal or greater number of brackets thanthe previous band (e.g., 54) configured respectively to correspond to aconcentric band (e.g., ring) of the same number of tubes of the tubebundle located in the thirteenth concentric band or ring of tubes. Suchtubes may be of the first size.

In an embodiment, a fourteenth circumferential band of the at least onetube support plate comprises an equal or greater number of brackets thanthe previous band configured respectively to correspond to a concentricband (e.g., ring) of the same number of tubes of the tube bundle locatedin the fourteenth concentric band or ring of tubes. Such tubes may be ofthe second size.

It will be apparent that any number of circumferential bands may beprovided.

In an embodiment, any of the circumferential bands of the at least onetube support plate further comprises brackets corresponding to at leastone thermocouple insertion tube, the at least one thermocouple insertiontube. Such thermocouple insertion tube may be similarly sized relativeto the tubes of the tube bundle (e.g., of the first or second size).

In an embodiment, at least four tube support plates are arrangedlongitudinally along the tube bundle.

In an embodiment, at least one tube support plate is arrangedlongitudinally along the tube bundle, wherein a circumferential band ofthe at least one tube support plate further comprises bracketscorresponding to at least one thermocouple insertion tube, wherein theat least one thermocouple insertion tube is configured to receive atemperature measurement device.

In an embodiment, the temperature measurement device is configured toobtain a temperature at a plurality of longitudinal locations within thereactor.

In an embodiment, the temperature measurement device is configured toobtain a temperature at a plurality of locations (e.g., at least eightdifferent locations), e.g., longitudinally along the reactor.

In an embodiment, the shell defines at least one flange facilitatingattachment and detachment of an upper portion of the shell from a mainbody portion of the shell.

In an embodiment, the shell is configured to attach to a skirt at abottom portion of the shell.

In an embodiment, the skirt defines an aperture configured to receive aninlet spool.

In an embodiment, the at least one tube support plate defines at leastone radial strut connected to at least one of a plurality ofcircumferential bands of the tube support plate, wherein the at leastone radial strut of the at least one tube support plate aligns axiallywith at least one radial strut of another tube support plate.

In an embodiment, the at least one radial strut of the at least one tubesupport plate is offset axially relative to at least one radial strut ofan adjacent tube support plate.

In an embodiment, the at least one tube support plate defines aplurality of radial struts arranged symmetrically about a longitudinalaxis of the reactor.

In an embodiment, the at least one tube support plate defines at leastone radial strut connected to at least one of a plurality ofcircumferential bands of the tube support plate, wherein the at leastone circumferential band of the at least one tube support plate isremovably secured to the at least one radial strut.

In an embodiment, at least one tube of the tube bundle defines a uniformthickness longitudinally within the reactor.

In an embodiment, at least one tube of the tube bundle defines a taperedthickness longitudinally within the reactor.

In an embodiment, at least one tube of the tube bundle is configured tofacilitate a greater degree of heat transfer proximate a bottom portionof the reactor relative to a top portion of the reactor.

In an embodiment, the reactor includes a shell defining an internalspace configured to receive a catalyst, where a domed head portion thatincludes a startup nozzle includes a flange for detachable connection toa reducing flange. The startup nozzle includes a manhole access openingthrough which a maintenance worker can enter the shell of the reactor.The reactor also includes an inlet nozzle, and a tube bundle including aplurality of tubes arranged in concentric bands about a longitudinalaxis of the reactor.

In an embodiment, the domed head portion is integral with the shell(e.g., all formed from a single piece of material), without anyconnecting flanges therebetween. Such a configuration reduces the flangearea, reducing any potential leakage points, provides a simplifieddesign, and reduces costs. Such a reduction in the flange diameter (sothat the flange has a diameter of just that required for the manholeaccess opening, e.g., about 40-80 cm) also ensures that the top portionof the reactor attached to the shell at such a flange is lighter weight,and easier to handle, manufacture, and maintain, as compared to aconfiguration where the entire domed head portion is separately flanged,to the reactor shell (e.g., which may require a significantly largerdiameter flange, such as approximately 2 meters).

In an embodiment, the domed head portion includes at least onethermocouple port, where the thermocouple port is at a tilted anglerelative to the longitudinal axis of the reactor (e.g., tilted relativeto vertical).

In an embodiment, the domed head portion includes two such thermocoupleports, each tilted relative to the longitudinal axis of the reactor.

In an embodiment, the reactor includes a shell defining an internalspace configured to receive a catalyst, at least one inlet nozzle, and atube bundle comprising a plurality of tubes arranged in concentric bandsabout a longitudinal axis of the reactor. The reactor further includes acatalyst support plate including a plurality of apertures formedtherethrough through which the plurality of tubes of the tube bundlepass. Each tube also passes through a plurality of tube support plates,positioned above the catalyst support plate. A support ring is attachedaround each tube passing through a corresponding aperture of thecatalyst support plate and the tube support plates, where the tubes arenot fixed (e.g., welded) relative to the catalyst support plate or thetube support plates, to allow for thermal expansion of the tubes passingthrough the catalyst support plate and tube support plates.

In an embodiment, each tube includes an upper support ring and a lowersupport attached to and extending around each of the tubes, at thelocation where each tube passes through the catalyst support plate, aswell as the location of passage through each tube support plate. Theupper support ring is positioned above the corresponding catalystsupport plate or tube support plate and the lower support ring ispositioned below the corresponding catalyst support plate or tubesupport plate, where a spacing between the upper and lower support ringsattached to a given tube is greater than a thickness of thecorresponding catalyst support plate or tube support plate. This permitsthe tube to slide within the aperture of the plate, to accommodatedifferential thermal expansion that may occur with different tubes,relative to the plates.

In an embodiment, the reactor includes a shell defining an internalspace configured to receive a catalyst, at least one inlet nozzle, and atube bundle comprising a plurality of tubes arranged in concentric bandsabout a longitudinal axis of the reactor. At least one tube supportplate is also provided, each tube support plate including a plurality ofapertures formed therethrough. Each tube of the plurality of tubes ofthe tube bundle passes through a corresponding one of the apertures inthe tube support plate. The reactor further includes at least onesliding strip at a periphery of the tube support plate(s), wherein atleast one of the tube support plates includes a slot formed at aperiphery of the tube support plate, for receipt of a correspondingsliding strip. In an embodiment, each tube support plate may includesuch a slot.

In an embodiment, each sliding strip further includes its own slot oropening, for receipt of a thickness of the corresponding tube supportplate, where a height of the opening in the sliding strip is greaterthan a thickness of the corresponding tube support plate. Such aconfiguration allows the sliding strip to slide up or down relative tothe tube support plate, with the tube support plate trapped within theopening of the sliding strip. The distance associated with the height ofthe opening determines how far the strip may slide, relative to the tubesupport plate. Such a sliding strip also simplifies assembly of thereactor and tube bundle.

In an embodiment, the at least one tube support plate includes a toptube support plate and one or more intermediate tube support, plates,positioned below the top tube support plate. As described herein, a topplate can also be provided in addition to the top tube support plate.The opening of the sliding strip that corresponds to the top tubesupport plate has a height that is approximately equal to the thicknessof the top tube support plate, so that the top tube support plate isfixed relative to the sliding strip. The openings of the sliding stripconfigured for receipt of the additional tube support plates (below thetop tube support plate) are sized larger than the opening associatedwith the top tube support plate, so that the sliding strip is slidablerelative to the additional tube support plates.

Any of the features noted above, or other features described herein maybe used in combination with one another, alone, or in combination withother features.

Other methods, embodiments, and variations of the system are describedin greater detail in the following discussion.

BRIEF DESCRIPTION OF THE DRAWINGS

These and other features, aspects, and advantages of the presentinvention will become readily apparent and better understood in view ofthe following description, appended claims, and accompanying drawings.

FIG. 1A is a perspective view of a reactor according to embodiment ofthe present disclosure.

FIG. 1B is a rotated perspective view of the reactor according to theembodiment of FIG. 1A.

FIG. 2 is a plan view of the reactor according to the embodiment of FIG.1A.

FIG. 3 is a cutaway elevational view of the reactor and reactorinternals of the embodiment of FIG. 1A taken along the line 1A-1A.

FIG. 4 is a cutaway elevational view of the reactor and catalyst bed andcatalyst support layers of the embodiment of FIG. 1A taken along theline 1A-1A.

FIG. 5A is a close-up elevational cutaway view of the reactor of theembodiment of FIG. 1A according to the detail IV.

FIG. 5B is a close-up elevational cutaway view of the reactor of theembodiment of FIG. 1A according to the detail III.

FIG. 6 is a perspective view of a tube bundle for use with a reactoraccording to the embodiment of FIG. 1A.

FIG. 7 is an elevational view of the tube bundle of the embodiment ofFIG. 6 .

FIG. 8 is a perspective view of a tube bundle and tube support plateaccording to the embodiment of FIG. 6 .

FIG. 9 is a plan view of a top and feed tube support plate according tothe reactor of the embodiment of FIG. 1A.

FIG. 10A is a plan view of the tube support plate according to theembodiment of FIG. 6 .

FIG. 10B is a plan view of a tube support plate according to anotherembodiment.

FIG. 11 is a plan view of a gas inlet plate according to the reactor ofthe embodiment of FIG. 1A.

FIG. 12 is a plan view of a catalyst support plate according to thereactor of the embodiment of FIG. 1A.

FIG. 13 is a close-up plan view of a catalyst support plate according tothe detail XII.

FIG. 14 is a perspective exploded view of a top plate and reactoraccording to the embodiment of FIG. 1A.

FIG. 15 is a plan view of the top plate of the embodiment of FIG. 14 .

FIG. 16 is a close-up perspective exploded view of a top plate for usewith the reactor of the embodiment of FIG. 1A according to the view XIV.

FIG. 17 is an elevational cutaway view of a retaining plate for use witha nozzle of a reactor according to the embodiment of FIG. 1A taken alongthe line 16A-16A.

FIG. 18 is an elevational view of the retaining plate and nozzleaccording to the embodiment of FIG. 17 .

FIG. 19 is a perspective view of the retaining plate and nozzleaccording to the embodiment of FIG. 17 .

FIG. 20 is a cutaway elevational view of a reactor, catalyst bed, andthermocouple insertion tube according to another embodiment,

FIGS. 21A-21B are perspective views similar to FIGS. 1A-1B, but for analternative reactor configuration.

FIG. 22 shows a cut-away elevational view similar to that of FIGS.5A-5B, but for the alternative reactor configuration of FIGS. 21A-21B.

FIG. 23 shows a cut-away elevational view of the alternative reactorconfiguration.

FIG. 24 shows an devotional view of a tube bundle, similar to that shownin FIG. 7 , but which includes a sliding strip at the periphery of thetube bundle and tube support plates.

FIG. 25 shows a top plan view of an exemplary top feed tube supportplate, similar to that shown in FIG. 8 , but which includes slots for asliding strip.

FIG. 26 shows a top plan view of that may be used for additionalexemplary feed tube support plates, also including slots for a slidingstrip.

FIG. 27 shows a detail of an exemplary slot, such as that included inthe support plates of FIGS. 25 and 26 .

FIG. 28 shows a detail of the support plate of FIG. 26 .

FIG. 29 shows a detail view, showing support rings attached to the feedtubes, and also showing the slot for the sliding strip, and the slidingstrip itself.

FIG. 30 shows an exemplary configuration for the sliding strip.

FIG. 31A shows engagement between the sliding strip, and the top tubesupport plate.

FIG. 31B shows engagement between the sliding strip, and an intermediatetube support plate, while also showing the position of the support ringsattached to the feed tubes, relative to the slots within the slidingstrip 220.

FIG. 31C shows engagement between the sliding strip, and the lowest tubesupport plate.

DETAILED DESCRIPTION OF VARIOUS EMBODIMENTS

A better understanding of different embodiments of the invention may behad from the following description read with the accompanying drawingsin which like reference characters refer to like elements.

While the disclosure is susceptible to various modifications andalternative constructions, certain illustrative embodiments are shown inthe drawings and will be described below. It should be understood,however, there is no intention to limit the disclosure to theembodiments disclosed, but on the contrary, the intention is to coverall modifications, alternative constructions, combinations, andequivalents falling within the spirit and scope of the disclosure anddefined by the appended claims.

It will be understood that, unless a term is defined in this patent topossess a described meaning, there is no intent to limit the meaning ofsuch term, either expressly or indirectly, beyond its plain or ordinarymeaning.

Turning to FIG. 1A, a reactor 100 according to embodiments of thepresent disclosure is shown. The reactor 100 comprises a shell 102defining an internal space 103 (FIG. 4 ) and comprising at least oneinlet nozzle 120. The reactor 100 is configured to receive and cooperatewith at least one reactor internal component, such as a tube bundle 130(FIG. 3 ) comprising one or more tubes 131. The reactor 100 extendslongitudinally about an axis 1A-1A from a top end 105 to a bottom end107 and may define a substantially cylindrical shape.

The inlet nozzle 120 is arranged generally proximate the bottom end 107such that one or more reactants may enter through the inlet nozzle 120and then travel upwardly in a direction F1 (FIG. 4 ) through theinternal space 103 of the reactor 100 within the one or more tubes 131before exiting the tubes 131 proximate the top end 105 and divertingdownward in a direction F2 toward an outlet nozzle 124 which defines acorresponding flange 125. As the reactants travel upwardly through theone or more tubes 131, the reactants exchange heat with the catalyst andthe reactants and products traveling downwardly in the direction F2(FIG. 4 ).

In exothermic reactions such as methanol synthesis, the reactantsadvantageously absorb heat generated by the reaction within the tubes131 to pre-heat the reactants prior to delivering the reactants to acatalyst bed 140. This also advantageously mitigates the formation ofcatalyst hotspots and associated catalyst sintering and productdegradation. This also reduces the likelihood of a runaway reaction, asthe reactants define a heat exchange medium for removing heat from thecatalyst bed. Due to the distribution of the tubes 131, the reactantsform a much more effective heat-exchange modality than, for example, acooling-water sleeve surrounding the reactor 100.

The reactor 100 may define, in addition to the inlet nozzle 120 and theoutlet nozzle 124, one or more catalyst unloading nozzles 116 and/or oneor more hand holes 118 through which the internal space 103 isaccessible. The one or more catalyst unloading nozzles 116 may be angleddownwardly so as to facilitate gravity-based removal of the catalyst,from the catalyst bed 140, for example when removing and rechargingspent catalyst. The one or more hand holes 118 may facilitatemaintenance by allowing a technician to insert a hand, tool, orinstrument into the internal space 103 proximate the catalyst supportplate 154, the catalyst bed 140, or at any other suitable location.

As seen in FIGS. 1A and 1B, the reactor 100 defines a startup nozzle 110configured for the provision of a heating fluid. During a startupoperation, when the reaction has not yet reached steady-state operation,the reactants may not receive a necessary amount of pre-heat as theytravel in the direction F1 in the tube bundle 130. The startup nozzle110 may receive a heating fluid such as an inert gas, like heatednitrogen gas, that may pass through the internal space 103 and providesenough enthalpy to achieve steady-state operation without adverselyaffecting the yield of the reaction.

The shell 102 further may define at least one thermocouple port 106.Each thermocouple port 106 may facilitate the insertion of a temperaturemeasurement device into the reactor 100 and in embodiments into the tubebundle 130 in an axial or longitudinal direction. By positioning thethermocouple port 106 at a top portion 105 of the reactor 100, a singletemperature measurement device, such as a thermocouple, may be insertedtherethrough with the ability to measure temperature at a plurality oflocations. In embodiments, the temperature measurement device may extendin an elongate manner and comprise a plurality of measurement devicessuch as thermocouples thereon at predetermined distances such that thereactor conditions at each of said predetermined distances may bemeasured for improved control of the reaction.

While two thermocouple ports 106 are shown in FIGS. 1A and 1B onopposite sides of the startup nozzle 110, it will be appreciated thatmore or fewer thermocouple ports 106 may be provided at any suitablelocation. By providing the temperature measurement devices through thethermocouple ports 106, the reactor 100 advantageously allows formeasurement of reactor conditions at different elevational locations inthe reactor while minimizing the number of thermocouple joints, therebyfacilitating improved process control and throughput while minimizingthe risk of leaks, either into or out of the shell 102. The location ofthe thermocouple ports 106 further allows for sampling the reactorconditions at desired radial locations of the reactor 100 regardless ofthe size of the reactor 100, in contrast to existing reactor designs inwhich the thermocouples are inserted radially, such that larger reactorsare sampled disproportionately close to the shell.

Turning to FIG. 4 , the shell 102 may define an inlet nozzle 120 with acorresponding flange 121 arranged a distance below a gas inlet plate 156and both arranged proximate the bottom end 107 of the reactor 100. Theinlet nozzle 120 may be arranged transverse relative to a longitudinalextension direction of the reactor 100, such that as the reactants enterthrough the inlet nozzle 120 in a flow direction F4, the reactantschange direction and enter into one or more tubes 131 of the tube bundle130 through the gas inlet plate 156 in the direction F1.

The inlet nozzle 120 may be arranged as shown to optimize a distancebetween the inlet nozzle 120 and a bottom of the tube bundle 130 and toevenly distribute the reactants to the tubes 131 such that eddies thatresult in blockages, hot spots, and uneven flow are avoided. The flange121 may be configured to facilitate attachment of a reactant feed lineto the nozzle 120. While the inlet nozzle 120 has been shown anddescribed, it will be appreciated that the distance between the inletnozzle 120 and the bottom of the tube bundle 130 may be greater orsmaller as suitable.

Additionally or as an alternative, the shell 102 further defines asecondary inlet nozzle 132 with a corresponding flange 133 as shown inFIG. 5A. The flange 133 may be configured to facilitate attachment of areactant feed line to the nozzle 132. The secondary inlet nozzle 132 isarranged to deliver the reactants vertically in a direction F3, whichmay correspond to or be parallel with the flow direction F1 upwardlythrough the tubes 131. The reactor shell 102 may be secured with a skirt108 which may define through a thickness thereof an aperture 122configured to receive an inlet spool 135 connecting to the secondaryinlet nozzle 132.

The skirt 108 may be cylindrical in shape and extend substantiallycoextensively with the reactor shell 102 downwardly from the bottom end107. The skirt 108 may define a ring 109 at grade securing the reactor100 and the skirt 108 in position. The inlet spool 135 may be curvedsuch that the reactants are fed toward the reactor 100 in a flowdirection generally transverse to the flow direction F3, for example ina direction substantially parallel to the direction F4 of the inletnozzle 120. The inlet nozzle 120 and the secondary inlet nozzle 132 maybe configured to operate simultaneously or independently of each other.While a skirt has been shown and described, any suitable support may beutilized, and the disclosure is not limited to the use of a skirt.

In embodiments, a diverter 137 may be removably arranged within thesecondary inlet nozzle 132 or the shell 102 for directing a flowdirection of the reactants when the secondary inlet nozzle 132 is inuse. The diverter 137 may define a shape that distributes a portion ofthe flow of reactants from the secondary inlet nozzle 132 radiallyoutward such that the flow is evenly distributed between the centraltubes, which are generally aligned with the secondary inlet nozzle 132,and outer tubes. While the diverter 137 has been shown and described, itwill be appreciated that any suitable structure, configuration, orarrangement may be utilized. In embodiments, the diverter 137 defines aplurality of apertures and/or protrusions configured for distributingthe flow of the reactants entered through the nozzle 132.

Turning to FIG. 5B, the reactor 100 may further comprise a domed headportion 104 that is detachable from the shell 102 and is releasablyattached thereto at flanges 112, 114 which may comprise any suitablemodality for attaching the domed head portion 104 and the shell 102,such as apertures and corresponding fasteners. The domed head portion104 may define a space 113 above a top extent of the tube bundle 130.The space 113 provides a space for the pre-heated reactants to mix anddivert back downwardly through the catalyst bed 140. The nozzle 110 maybe defined through a thickness of the domed head portion 104 to allowfor the addition of a heating medium during start-up operation, asdescribed previously.

While a domed head portion releasably securable to a shell has beenshown and described, it will be appreciated that the disclosure is notlimited thereto, and for any size of reactor, a fixed head, for examplecomprising a flanged manhole, may be utilized instead.

The thermocouple ports 106 may be aligned with respective thermocoupleinsertion tubes 126, which may extend a distance above the top extent ofthe tube bundle 130. The thermocouple ports 106 may extend through apart or an entirety of a thickness of the domed head portion 104 toallow access to the reactor interior 103. The thermocouple ports 106 mayfacilitate access to the reactor interior 103 in any suitable way, suchas by defining an aperture of a size that is configured to be flush witha surface of the temperature measurement device such that pressure maybe maintained within the reactor interior 103, by cooperating with agasket seal, combinations thereof, or any other suitable means. Anysuitable modality may be used. By extending a distance above the topextent of the tube bundle 130, the thermocouple insertion tubes 126 areconfigured to be more easily identified during installation of thethermocouple, particularly as access is limited when the domed headportion 104 is in place. The thermocouple insertion tubes 126 may extendalong a length of the reactor 100 substantially parallel to or alignedwith the feed tubes 131.

The reactor 100 further may comprise one or more of a catalyst supportplate 154, at least one tube support plate 162, 163, 164, 165, a gasinlet plate 156, a top and feed tube support plate 150, and/or a topplate 190, the provision of which advantageously facilitates securingthe tube bundle 130 within the shell 102 while allowing for access tothe reactor interior 103 as necessary for maintenance or other purposes.The gas inlet plate 156 and the catalyst support plate 154 mayadvantageously be welded to an interior surface of the shell 102 tosecure the tube bundle 130 therewithin.

The tubes 131 of the tube bundle 130 may be welded to the gas inletplate 156, the top and feed tube support plate 150, and/or to the atleast one tube support plate 162, 163, 164, 165. In embodiments, onlythe gas inlet plate 156 is welded or otherwise secured to the interiorsurface of the reactor shell 102, with the top and feed tube supportplate 150 and the at least one tube support plate 162, 163, 164, 165being unsecured so as to accommodate thermal expansion of the tubes 131.

Turning to FIG. 4 , the catalyst bed 140 may comprise one or moresections of catalyst, such as solid catalyst. The catalyst bed 140 mayalso or alternatively comprise one or more inert sections 142, 144,which sections may comprise support ceramic balls of a first diameter,such as 1-30 mm, more specifically 5-20 mm, or in embodiments 9 mm. Thecatalyst bed 140 may also comprise support ceramic balls of a seconddiameter, such as 1-30 mm, more specifically 10-25 mm, or in embodiments19 mm. The catalyst bed 140 may define distinct sections 142, 144corresponding to ceramic balls comprising substantially only balls of asingle size.

For example, in the depicted embodiment the section 142 comprisessubstantially only balls having a diameter of 9 mm while the section 144comprises only balls having a diameter of 19 mm. The sections 142, 144may have any suitable height within the reactor 100, such as 5-500 mm,more specifically 100-300 mm, or in embodiments 200 mm for each of thesections 142, 144. The height of sections 142, 144 may the same, ordifferent from one another. The catalyst bed 140 may additionally oralternatively comprise solid catalyst having a shape defining at leastone of pellets, rings, tablets, or spheres. The sections 142, 144 may bearranged proximate (e.g., above, or directly above) the catalyst supportplate 154 and below a section 141 comprising substantially only solidcatalyst of a different shape and/or size than the support ceramic ballsof sections 142, 144.

The support ceramic balls sections 142, 144 advantageously support aweight of the catalyst in the catalyst bed while promoting effective andeven flow distribution. By providing distinct first and second sections142, 144, the flow of reactants, products, and byproducts through thereactor interior 103 toward the outlet nozzle 124 is improved as theflow of gases is allowed between the catalyst particles in the catalystbed 140, between the support ceramic balls of the first, smallerdiameter in the first section 142, and finally between the supportceramic balls of the second, larger diameter in the second section 144prior to passing through the catalyst support plate 154. The supportceramic balls may advantageously be inert and configured to resistthermal shock and corrosion from various reactants, products, and/orbyproducts. While support ceramic balls have been described, it will beappreciated that the sections 142, 144 may have more or fewer sectionsand may comprise differently shaped or sized support structures, such asrings, cylinders, polygons, or otherwise.

In embodiments, the section 141 of the catalyst bed 140 may have ordefine a first height 148 corresponding to an unreduced catalyst height,and a second height 146 corresponding to a reduced catalyst height.

While the section 141 of the catalyst bed 140 may comprise catalystparticles of a single size and/or shape, it will be appreciated thatdistinct sections within the catalyst bed 140 of differently sizedand/or shaped catalyst particles are contemplated within the scope ofthe present disclosure. The catalyst particles may have any suitableshape or configuration, such as spheres, pellets, cylinders, trilobes,quadralobes, pyramids, cones, stars, or otherwise, and may have anysuitable number and size of apertures defined therethrough and/ornotches or grooves defined on a portion of the surface thereof. Distinctsections corresponding to a single, different type of catalyst sizeand/or shape may be provided in the catalyst bed 140, for example asaxial or radial layers or pockets. In embodiments different sizes andshapes of catalyst particles may be provided and mixed together withinthe catalyst body in any suitable configuration.

The catalyst particles in the catalyst bed 140 may be a function of andcooperative with the support ceramic balls in the sections 142, 144, orvice versa. In embodiments the catalyst particles are selectedindependently of the support ceramic balls.

A tube bundle 130 according to an embodiment is shown in FIGS. 6 and 7 .The tube bundle 130 is configured to extend substantially longitudinallyabout the axis 1A-1A within the shell 102 and is maintained by, in orderfrom top to bottom, a top plate and tube support plate 150, a pluralityof tube support plates 162, 163, 164, 165, a catalyst support plate 154,and a gas inlet plate 156. A distance 161 between the top plate and tubesupport plate 150 and the tube support plate 162 and between the tubesupport plates 162, 163, 164, and 165 may be uniform along a length ofthe tube bundle 130. In embodiments the distance 161 may vary. Adistance 167 between the tube support plate 165 and the catalyst supportplate 154 may be greater than the distance 161. A distance 169 betweenthe catalyst support plate 154 and the gas inlet plate 156 may besmaller than the distance 167. It will be appreciated that the depictedembodiment is merely exemplary and any arrangement of the tube bundle130 may be used.

The tubes 131 may define a uniform thickness and diameter along alongitudinal length of the tube bundle 130. In embodiments, the tubes131 have a tapered thickness along the length of the tube bundle, withincreased thickness and/or diameter proximate one or more of the plates150, 162, 163, 164, 165, 154, 156 in order to support the plates. Inembodiments, one or more of the tubes 131 of the tube bundle 130 mayhave an increased thickness relative to other tubes 131 for increasedstructural support. For example, tubes 131 that extend closer to acenter or an outer edge of the tube bundle 130 may have an increasedthickness relative to the other tubes of, for example, 10%, 20%, 25%,33%, 50%, or any other suitable thickness. That is, the walls of suchtubes 131 may have an increased thickness while in embodimentsmaintaining a same internal diameter. This advantageously allows thetubes 131 with the increased thickness to convey reactants whilesupporting the tube bundle 130, thereby freeing up cross-sectional areafor increased catalyst loading and more evenly distributed catalystrelative to other structural arrangements.

In embodiments, the tubes 131 have a reduced thickness and/or increaseddiameter proximate a bottom portion of the reactor 100, for example tofacilitate more-efficient heat transfer at the bottom portion of thereactor 100 compared to the top portion of the reactor 100.Alternatively, one or more of the tubes 131 of the tube bundle 130 maycomprise internal tube rods configured to increase a velocity of thereactants being preheated therein. The internal tube rods may extend apartial or entire distance from a bottom of the tubes 131 to a top ofthe tubes 131.

The tube bundle 130 and the reactor 100 generally are advantageouslyconfigured for modularity in design and implementation. Whereas existingshell-and-tube-type reactors are not easily scalable due to thesignificant rework that must be completed to properly balance the tubelength and diameters, the catalyst bed, the shell, and other components,the design of the reactor 100 advantageously allows for scaling up ordown based on the arrangement of the concentric bands of tubes 131 onthe tube bundle 130. The tube bundle 130 is arranged such that whethercircumferential bands of tubes 131 are added (to increase the capacityof the reactor design for larger throughput or during a debottleneckeffort) or removed (for scaling down the capacity of the reactordesign), other geometric features of the reactor may remain unchanged.As a result extensive redesign work can be avoided.

The tube bundle 130 may be configured such that one or more geometricconstraints or ratios are maintained in any design, regardless ofwhether the reactor and tube bundle are configured for reducedthroughput or for increased throughput in various designs. To ensurethat a tube density is improved, an average tube pitch (i.e. acenter-to-center distance between tubes) of the tube bundle may besubstantially constant throughout the tube bundle, with thecircumferential bands and tubes defining the same being spaced so as tomaintain a constant tube pitch.

As another example, the tube bundle 130 advantageously achieves adesired ratio of a cumulative cross-sectional area of the catalyst bedwhen viewing the reactor according to a plan view relative to acumulative cross-sectional area of the tubes 131 (i.e. the total radialsurface area of the tubes taken together) according to the same planview. In embodiments, the ratio of the cumulative cross-sectional areaof the catalyst relative to the cumulative cross-sectional area of thetubes is in a range between 2 and 20, more specifically between 5 and12.

Regardless of a circumferential band of tubes 131 being added to orremoved from the tube bundle 130 design, the cross-sectional area of thetubes 131 relative to the catalyst bed may be simply and easily adjustedso as to remain within a suitable bound, such that the performance ofthe reactor, and in particular its safety profile, are suitable. In anembodiment, adding or removing one or more circumferential bands oftubes may not substantially change the cumulative cross-sectional areaof the catalyst relative to the cumulative cross-sectional area of thetubes. In other embodiments, the tube bundle 130 may be designed suchthat any other geometric or process-related parameter is targeted suchthat removal or addition of circumferential bands of tubes do not entailextensive redesign but rather allow an engineer to simply and easilyadjust the reactor to a new, required capacity or other requirement. Byproviding a tube bundle 130 with the specified relation between thecross-sectional areas of the tubes and the catalyst bed, heatdistribution is improved, which reduces the likelihood of runawayreactions by reducing hotspots and improving overall throughput throughthe reactor 100.

The reactor 100 may be controlled and maintained during operation tocontrol one or more features of the catalyst bed 140 and/or the tubebundle 130. In some embodiments, the reactor 100 is configured toutilize the temperature measurement devices to evaluate a distributionof heat throughout the cross-sectional area of the catalyst bed. Inparticular, the reactor 100 may be controlled by assessing a radialtemperature gradient within the reactor according to depth and/orassessing a growth of the gradient according to depth within the reactor100 (from the top end 105 toward the bottom end 107).

Turning to FIGS. 12 and 13 , the catalyst support plate 154 isconfigured to support a total height of the solid catalyst, such as aheight of the sections 142, 144 combined with the height of the section141. The catalyst support plate 154 further advantageously supportsforces due to differential pressure over the catalyst bed 140. Thecatalyst support plate 154 may be arranged within the shell 102proximate the catalyst unloading nozzle 116 and/or the hand hole 118.The catalyst support plate 154 may define one or more apertures 180,181. The apertures 180, 181 may comprise or define apertures comprisinga plurality of apertures of a first size corresponding to the apertures180 and a plurality of apertures of a second size corresponding to theapertures 181, the apertures extending through at least part of athickness of the catalyst support plate 154.

The first size of the apertures 180 may correspond to a circumference ofat least one tube 131 of the tube bundle 130. In embodiments, the firstsize of the apertures 180 is larger than a circumference of the tubes131 to allow for a degree of movement and/or thermal expansion of thetubes within the aperture 180. The apertures 180 may be defined throughthe catalyst support plate 154 according to an arrangement of theplurality of tubes 131 in the tube bundle 130. The second size of theapertures 181 may be smaller than the first size of the apertures 180,the second size of the apertures 181 serving to allow for flow ofreactants, reaction products, and reaction byproducts therethrough enroute to the outlet nozzle 124.

In embodiments, one or more of the apertures 180 may define a terminusfor a temperature measurement device. The apertures 182 may be sized andconfigured to receive a thermocouple insertion tube 126 and to terminatean extension of the thermocouple insertion tubes 126 (FIG. 7 ). Theapertures 182 may in embodiments extend only partly into the thicknessof the catalyst support plate 154. In embodiments the thermocoupleinsertion tubes 126 may be welded to the catalyst support plate 154 andplugged thereat. The tubes 131 may not be welded to the catalyst supportplate 154 to allow for the effects of thermal expansion.

The size of the apertures 181 and/or the average distance between theapertures 181 may be a function of the thickness of the catalyst supportplate 154, such that the size of the apertures 181 is proportional to athickness of the catalyst support plate 154 and/or the distance betweenthe apertures 181 is inversely proportional to the thickness of thecatalyst support plate 154. That is, the greater the thickness of thecatalyst support plate 154, the greater the diameter of the apertures181 and/or the smaller the distance between the apertures 181. Inembodiments, the catalyst support plate 154 may have a thickness ofbetween 20 and 500 mm, more specifically between 50 and 300 mm, and inembodiments 110 mm, while the apertures 181 may have a diameter of 1-50mm, more specifically 5-25 mm, and in embodiments 10 mm.

As seen in the close-up view of FIG. 13 , the apertures 180 may extendin a pattern or arrangement corresponding to an arrangement of tubes 131in the tube bundle 130 as will be discussed in greater detail herein.The apertures 181 may extend between each of the apertures 180. Theapertures 181 may define any suitable pattern or arrangement, such as anextension direction 183A and/or a transverse extension direction 183B,the extension directions 183A, 183B defining straight lines. Otherpatterns or arrangements of the apertures 181 are contemplated withinthe scope of the disclosure. The apertures 181 may be spaced apart fromeach other by any suitable distance, including in embodiments by adistance of 1-30 mm from center to center of adjacent apertures 181,more specifically from 5-20 mm from center to center, and in embodiments15 mm from center to center of adjacent apertures 181 along one or bothof the directions 183A, 183B. The distance from center to center ofadjacent apertures 181 need not be uniform across an entirety of thesurface of the catalyst support plate 154 but rather may vary assuitable.

The catalyst support plate 154 may define at an outer periphery a band184 of material forming the catalyst support plate 154 that does notdefine any of the apertures 180, 181. The band 184 may extend partiallyor wholly about the periphery of the catalyst support plate 154 andadvantageously facilitates welding or other suitable attachment of thecatalyst support plate 154 to the interior surface of the shell 102. Inembodiments, the band 184 may extend into and then be welded to a recessdefined by the inner surface of the shell 102. The band 184 may extendany suitable distance such as 5 mm radially.

Turning to FIG. 11 , the gas inlet plate 156 may be arranged below thecatalyst support plate 154, and may comprise a plurality of apertures155 defined through at least part of a thickness of the gas inlet plate156. The plurality of apertures 155 may be circular apertures definedthrough the gas inlet plate 156 according to the arrangement of theplurality of tubes 131 of the tube bundle 130, and aligning with anarrangement of the apertures 180 of the catalyst support plate 154. Inan embodiment, the gas inlet plate 156 is substantially solid and devoidof openings outside of the plurality of apertures 155 so as to force theincoming reactants into the tubes 131. The plurality of tubes 131 may beseal welded and/or strength welded to the gas inlet plate 156. It willbe appreciated that where a component is discussed herein as beingwelded to another component, seal welding, strength welding, acombination thereof, or any other type of attachment is contemplated.

Turning to FIGS. 8-9 , the reactor 100 may further comprise at least onetube support plate 150, 162, 163, 164, 165 which may be arrangedlongitudinally spaced apart along an axial or longitudinal length of atube bundle 130. The tube support plates 150, 162, 163, 164, 165 areshown and described, but it will be appreciated that more or fewersupport plates may be provided. The top and feed tube support plate 150may be substantially the same as the tube support plates 162, 163, 164,165 and may include or omit one or more features. For example, the topand feed tube support plate 150 may have the same features as the tubesupport plates 162, 163, 164, 165 and may further include one or morespacers configured to cooperate with a top plate, as will be describedin greater detail below.

The tube support plate 150, 162, 163, 164, 165 may comprise at least onecircumferential band 168 configured to maintain a position of the atleast one tube 131. The at least one circumferential band 168 comprisesat least one bracket 172 configured to extend about a portion of a tube131 of the tube bundle 130. In embodiments, the at least one bracket 172extends about an entirety of the tube 131. The bracket 172 may beconfigured to releasably attach to the tube 131.

In embodiments, the bracket 172 may extend about only a portion ratherthan an entirety of the tube. The bracket 172 may advantageouslycooperate with a beam 173 that extends between the bracket 172 and anadjacent bracket 172 attached to an adjacent tube 131. The bracket 172may be connected releasably or non-releasably with the beam 173 and maydefine a filleted connection, for example. A circumferential band 168may be defined by a series of connected brackets 172 and beams 173defining a substantially circumferential arrangement with correspondingtubes 131.

The circumferential band 168 may be concentrically arranged withadjacent circumferential bands 168 of the tube support plate 150, 162,163, 164, 165, with the circumferential bands 168 optionally centered onthe longitudinal axis 1A-1A of the reactor. The cooperation of brackets172, beams 173, radial struts 166, and circumferential bands 168together define a tube support plate. While the circumferential bands168 have been shown and described, It will be appreciated that anysuitable configuration may be used, including asymmetric, offset, ornon-circumferential arrangements. While the cooperation of variouscomponents is described as defining a tube support plate, it will beappreciated that a tube support plate may take any suitableconfiguration and is not limited hereby.

The at least one tube support plate 150, 162, 163, 164, 165 defines atleast one radial strut 166 connected to the at least one circumferentialband 168 at an attachment point 169 and/or to an outer support band 170at an attachment point 171. The tube support plate may define aplurality of radial struts 166 arranged radially symmetrically, forexample at 22.5° increments, at 30° increments, at 45° increments, at90° increments, at 120° increments, at 180° increments, anotherincrement evenly divisible by 360°, or otherwise. In other embodiments,the radial struts 166 are arranged asymmetrically in any suitablemanner.

The outer support band 170 may define a substantially continuous band ofsupport material, such as stainless steel, that provides sufficientrigidity, strength, and/or support to the tube support plate, and/orthat facilitates attachment of the outer support band 170 to an innersurface of the reactor shell 102. While eight radial struts 166 areshown and described regarding the embodiment of FIGS. 9 and 10 , it willbe appreciated that more or fewer radial struts 166 may be provided, andthat all of the tube support plates 150, 162, 163, 164, 165 need nothave a same number or arrangement of radial struts or other components.

The radial struts 166 may extend straight outwardly from a center of thetube support plate to the outer support band 170, or may define acurved, bent, tortuous, or other configuration. The radial struts 166may be formed of any suitable material, such as stainless steel, and maydefine heat-resistance properties to retain desired stiffness andstrength in the reactor conditions. The radial struts 166 advantageouslydefine attachment points 169 between the circumferential bands 168 andthe radial struts 166. The attachment points 169 may be releasable ornon-releasable, and may define any suitable connection, such as beingwelded together or being attached by a suitable fastener. The tubesupport plate may be configured to move with the tubes 131 by thermalexpansion and contraction, and may be formed of hightemperature-resistance materials, such as steel (e.g., stainless steel),ceramics, polymeric materials, composite materials, or otherwise.

In embodiments, the tube support plate 150, 162, 163, 164, 165 may befabricated using any suitable means. In embodiments, the tube supportplate 150, 162, 163, 164, 165 is formed from a single, solid plate fromwhich material is removed for example by water jet cutting. In otherembodiments, the radial struts and circumferential bands areindependently fabricated and assembled to form the tube support plates.

The top and feed tube support plate 150 may additionally define one ormore spacers 174 on a top surface thereof. The spacers 174 may beattached to one or more structures of the top and feed tube supportplate 150 in any suitable manner, including by welding. The spacers 174may extend a predetermined height and may define an aperture within acenter portion thereof. The aperture may comprise one or more threadingsconfigured to matingly engage with one or more threadings of a fastener,as will be discussed in greater detail herebelow regarding the top plate190. The spacers 174 may extend about the top and feed tube supportplate 150 in any suitable arrangement and in any suitable number.

For instance, the spacers 174 may define three concentric ring patterns175 (FIG. 9 ) about the top and feed tube support plate 150 as thespacers 174 attach to radial struts 166. In an embodiment, the spacers174 extend along four of the radial struts 166 between the first andsecond circumferential bands, between the seventh and eighthcircumferential bands, and between the thirteenth and fourteenthcircumferential bands. A total of four spacers 174 may be arranged oneach of the concentric ring patterns 175, such that a corner portion ofeach segment of the top plate 190 may be fastened thereto, as will bedescribed herebelow.

The arrangement of the radial struts 166 advantageously provides asecure attachment of the tubes 131 of the tube bundle 130 whileminimizing interference with the distribution of catalyst as thecatalyst is loaded from the top portion 105 of the reactor 100. Forexample, as the catalyst particles are poured into the shell 102, theradial struts 166 are configured to minimize uneven distribution of thecatalyst. In embodiments, the radial struts 166 of adjacent tube supportplates 162, 163, 164, 165 may align axially along the longitudinalextension length of the reactor 100.

In other embodiments, as shown in FIG. 10B, the radial struts 167 ofadjacent tube support plates may be offset from the radial struts 166 topromote even distribution of the catalyst during loading. The degree ofoffset may be any suitable degree. In embodiments, the radial struts 167are offset by a distance corresponding to half the angular distancebetween the radial struts 166. In the embodiment of FIG. 10B, the radialstruts 166 are offset by 45° from each other, and the offset of theradial struts 167 is 22.5°. Subsequent tube support plates may alternatein arrangement. The radial struts 166 of adjacent tube support platesmay be offset down a longitudinal length of the reactor so as to definea spiral or helix pattern. The depicted embodiment is exemplary, and anyother arrangement may be used as suitable.

The tube bundle 130 may be arranged such that an innermostcircumferential band 168A of the at least one tube support platecomprises six brackets configured respectively to correspond to a ringof six innermost tubes of a first size. The first size may be, forexample, 0.5-3 mm in diameter, more specifically 1-2 mm in diameter, andin embodiments 1.5 mm. A second circumferential band 168B of the atleast one tube support plate comprises 10 brackets configuredrespectively to correspond to a ring of 10 tubes of the tube bundle ofthe first size. A third circumferential band 168C of the at least onetube support plate comprises 14 brackets configured respectively tocorrespond to a ring of 14 tubes of the tube bundle of a second size.The second size may be, for example, 0.5-5 mm in diameter, morespecifically 1-4 mm, and in embodiments 2.5 mm.

A fourth circumferential band 168D of the at least one tube supportplate comprises 18 brackets configured respectively to correspond to aring of 18 tubes of the tube bundle of the first size. A fifthcircumferential band 168E of the at least one tube support platecomprises 22 brackets configured respectively to correspond to a ring of22 tubes of the tube bundle of the first size. A sixth circumferentialband 168F of the at least one tube support plate comprises 26 bracketsconfigured respectively to correspond to a ring of 26 tubes of the tubebundle of the first size.

A seventh circumferential band 168G of the at least one tube supportplate comprises 30 brackets configured respectively to correspond to aring of 30 tubes of the tube bundle of the second size. An eighthcircumferential band 168H of the at least one tube support platecomprises 34 brackets configured respectively to correspond to a ring of34 tubes of the tube bundle of the first size. A ninth circumferentialband 168I of the at least one tube support plate comprises 36 bracketsconfigured respectively to correspond to a ring of 36 tubes of the tubebundle of the first size. A tenth circumferential band 168J of the atleast one tube support plate comprises 42 brackets configuredrespectively to correspond to a ring of 42 tubes of the tube bundle ofthe first size.

An eleventh circumferential band 168K of the at least one tube supportplate comprises 46 brackets configured respectively to correspond to aring of 46 tubes of the tube bundle of the second size. A twelfthcircumferential band 168L of the at least one tube support platecomprises 50 brackets configured respectively to correspond to a ring of50 tubes of the tube bundle of the first size. A thirteenthcircumferential band 168M of the at least one tube support platecomprises 54 brackets configured respectively to correspond to a ring of54 tubes of the tube bundle of the first size. A fourteenthcircumferential band 168N of the at least one tube support platecomprises 58 brackets configured respectively to correspond to a ring of58 tubes of the tube bundle of the second size.

While the first through fourteenth circumferential bands have been shownand described, it will be appreciated that the reactor embodiments ofthe present disclosure advantageously facilitate a modular reactorconstruction that accommodates different throughput requirements ofdifferent facilities better than existing reactor designs. As needed,for example, an engineer may modify the depicted tube bundle 130 to havemore, fewer, and/or different circumferential bands. In order to scaleup the tube bundle 130 and the reactor 100 as a whole to accommodate ahigher yearly capacity of a plant, such as during a debottleneckingeffort, an additional circumferential band may be added to increase thenumber of tubes and expand the tube bundle outwardly in a simplemodification. For example, the attachments 171 between the radial struts166 and the outer band 170 may be released such that an additionalcircumferential band may be added to the tube support plate, with theouter band 170 replaced about the new circumferential band. To this end,the outer band 170 may be configured to have an expandablecircumference.

Conversely, to scale down the reactor 100, a circumferential band, suchas an outermost circumferential band, may be removed to reduce the sizeof the tube bundle so as to fit a smaller reactor shell and/or to yielda correspondingly lower yearly plant capacity. This may be done, forexample, by detaching the attachments 169 between circumferential bandsand the radial struts.

Moreover, the arrangement of the circumferential bands as shown allowsfor the addition or removal of circumferential bands and theaccompanying brackets and tubes while accommodating the structure of theradial struts. As seen, the circumferential bands increase in number ofbrackets and tubes such that the tubes are positioned in a substantiallyeven distribution and with sufficient space between the tubes to allowfor catalyst and reactant to pass therebetween and for thecircumferential bands to be added or removed without disrupting thedesign of the radial struts and the tube support plate generally.

In an embodiment, the ninth circumferential band 168I (or any other) ofthe at least one tube support plate further comprises brackets 172corresponding to at least one thermocouple insertion tube 126, the atleast one thermocouple insertion tube 126 being of the first tube size.The provision of brackets 172 for the thermocouple insertion tube 126allows for temperature measurement devices to be inserted into the tubebundle, preferably into a region of the tube bundle where thetemperature measurement device will be surrounded by catalyst and tubes,for accurate temperature readings along a longitudinal length of thereactor.

The top and feed tube support plate, similar to the tube support plates162, 163, 164, 165, may comprise one or more radial struts 166, an outerband 170, and one or more brackets 172 configured to engage with and/orsurround a tube 131 of a tube bundle 130. The radial struts 166 of thetop and feed tube support plate 150 may be arranged analogous orcorresponding to the struts 166 of the feed tube support plates 162,163, 164, 165 and may be divided axially by a suitable angle 176 (FIG. 9), such as 45°. It will be appreciated that other angles or arrangementsare contemplated by the present disclosure.

The brackets 172 of the top and feed tube support plate 150 mayconstitute or extend proximate a terminus of the tubes 131, with thepre-heated reactants exiting the tubes 131 thereat and then flowing inthe second direction F2 downwardly. The thermocouple insertion tubes 126may extend a distance above a topmost distance or extent of the tubes131, this facilitating easier insertion of the temperature measurementdevices from the thermocouple port 106 to the thermocouple insertiontube 126. As with the tube support plates 162, 163, 164, 165, the topand feed tube support plate 150 may be configured to be expanded ordecreased in size as suitable for a desired capacity of the reactor 100.

The arrangement of the tube bundle 130 and the tube support plates 150,162, 163, 164, 165 may advantageously account for heat transfer andreactor kinetics of the reactor.

Turning to FIGS. 14-16 , a top plate 190 is shown. The top plate 190 maybe configured to be installed atop or above the top and feed tubesupport plate 150. The top plate 190 may be modular in construction anddefine four distinct segments 192 surrounded by a flange 191. The topplate 190 may define a plate edge 194, one or more tube holes 202defined through at least a partial thickness of the plate 190, and oneor more gas apertures 204 defined through at least a partial thicknessof the plate 190. The tube holes 202 may be configured to aligngenerally with an arrangement of the tubes 131 of the tube bundle 130and facilitate passage of pre-heated reactants out of the tubes 131 intothe space 113 (FIG. 5B) of the reactor 100.

The gas apertures 204 facilitate passage of the pre-heated reactant intothe catalyst bed 140 and ensure proper flow distribution. The top plate190 may be configured to create a small pressure drop to make the flowentering the catalyst bed as uniform as possible. The top plate 190 isadvantageously configured to achieve improved uniformity of flowdistribution using a simplified design as shown and described relativeto existing approaches which may utilize heavy and/or complicateddesigns that are difficult and/or costly to manufacture and/or tomanipulate for maintenance purposes.

As the top plate 190 may extend outwardly to the flange 191, the gasapertures 204 may extend substantially to the edge 194 without leaving agap as in the catalyst support plate 154. The top plate 190 may have areduced thickness compared to the catalyst support plate 154. Inembodiments, the top plate 190 has a thickness of between 1 and 25 mm,more specifically between 5 and 15 mm, and in embodiments 8 mm.

The top plate 190 is configured to be removably attached to the shell102 and/or to the top plate and tube support plate 150 by any suitablemechanism, such as by the use of fasteners 196 that cooperate withcorresponding apertures 193 (FIG. 15 ) at the edge of each section ofthe plate 190. The fasteners 196 of the top plate 190 may cooperate withone or more of the spacers 174 extending between the top plate 190 andthe top and feed tube support plate 150, and which may be welded, forexample tack welded, to the top and tube support plate 150.

In embodiments, the spacers 174 may have a height and/or circumferencesufficient to receive a mating end of the fastener 196 within a track orrecess defined through a portion of a thickness of the spacer 174, thisallowing a robust attachment of the top plate 190 onto the top and feedtube support plate 150. The height of the spacer 174 may be between 1and 30 mm, more specifically between 5 and 20 mm, and in embodiments 15mm. The spacer 174 may be welded onto a radial strut 166, acircumferential band 168, a bracket 172, or otherwise. As seen, thefasteners 196 and the corresponding spacers 174 may be located such thata fastener and spacer 196, 174 is provided in each corner and alonginterior edges of a section 194 of the top plate 190.

The top plate 190 may further comprise or cooperate with one or moreload rings 195. The load rings 195 may be any suitable componentconfigured to facilitate positioning and/or removal of the section 194of the top plate 190. The load rings 195 may attach through one or moreof the gas apertures 204 or at any other suitable location and define acomponent for removably securing to and manipulating the top plate 190.In embodiments the load rings 195 are configured to allow an operator tograsp the top plate 190 with a tool for lifting the top plate 190 awayfrom the reactor shell 102.

By providing the top plate 190 in a modular fashion, with the distinctsections 194, the top plate 190 is more easily removable and replaceableduring maintenance operations without sacrificing the ability of the topplate 190 to distribute the reactants and secure the catalyst bed 140.The modular construction of the top plate 190 further makes themanufacturing process less costly and complex, as identical sections 192may be manufactured rather than plates 190 of unitary construction. Onebenefit of the arrangement of the top plate 190 is the ability for aplant worker to stand on one of the sections 194 of the top plate 190while loading catalyst through the opening provided by a section 194that has been removed.

Turning to FIGS. 17-19 , a retaining plate 210 for use with one or morenozzles of the reactor 100 is shown and described. The retaining plate210 may secure the catalyst unloading nozzle 116 and/or the hand hole118. The retaining plate 210 may comprise a handle 212 and is configuredto cooperate with a lip 214 defined by the nozzle 116. In embodiments,the nozzle 116 defines a plurality of lips 214 arrangedcircumferentially about an opening of the nozzle in any suitablepattern, with the retaining plate 210 configured to abut an innersurface of the lip 214 as seen in FIG. 17 . In embodiments, the lips 214are spaced apart by an angle, such as 15°, 20°, 30°, 45°, 60°, 90°, orotherwise. The arrangement of the lips 214 may be symmetric orasymmetric. The flange 117 of the nozzle 116 may define one or moreapertures 211 through which suitable fasteners may be received toconnect the nozzle 116 to a suitable spool.

In particular embodiments, the plurality of lips 214 do not extend abouta bottommost section B of a circumferential aperture defined by thecatalyst unloading nozzle 116 or the hand hole 118. Rather, as seen inFIG. 19 , the bottommost section B is unobstructed such that catalystparticles may flow freely under the effects of gravity during catalystunloading. The arrangement of the retaining plate 210 advantageouslyprevents the catalyst from flowing too fast during catalyst unloading.

Turning to FIG. 20 , a reactor 300 according to an embodiment is shownand described. The “300” series reference numbers may include similar oridentical features to those already described with “100” seriesreference numbers. The reactor 300 comprises a shell 302 in which a tubebundle having a top plate 350 as described above may be received andsecured, and defines an inlet nozzle 320 and an outlet nozzle 324. Theshell 302 may further comprise or cooperate with a domed top portion 304defining and/or supporting a thermocouple insertion nozzle 306. Thedomed top portion 304 may be secured to the shell 302 by a flange 312.The reactor 300 extends longitudinally about an axis 20A-20A. A catalystbed 340 may extend a suitable height within an internal space defined bythe reactor shell 302.

The reactor 300 further defines a thermocouple insertion tube 326extending about or substantially parallel or aligned with thelongitudinal axis 20A-20A and through the catalyst bed 340. Thethermocouple insertion tube 326 may be integrated with or independent ofa tube bundle as described above. The thermocouple insertion tube 326 isconfigured to receive a temperature measurement device 310, whichlikewise extends about the longitudinal axis 20A-20A. The temperaturemeasurement device 310 may be a multi-element thermocouple. Themulti-element thermocouple is configured to obtain a measurement of atemperature at a plurality of locations along the reactor 300.

As seen in FIG. 20 , the temperature measurement device 310 may compriseeight measurement locations 382A, 382B, 382C, 382D, 382E, 382F, 382G,382H along the length of the reactor 300 and extends to a terminus 327.The temperature measurement device 310 may have a total length 3301. Thelocations 382A, 382B, 382C, 382D, 382E, 382F, 382G, 382H may bedistanced by, respectively, distances 330A, 330B, 330C, 330D, 330E,330F, 330G. The distances 330A, 330B, 330C, 330D, 330E, 330F, 330G maybe a same distance such that the measurement locations are evenly spacedalong the reactor 300, or may be different distances depending on theneeds of a particular process.

The thermocouple insertion tube 326 may be suitably configured to allowthe temperature measurement device 310 to obtain readings at thelocations 382A, 382B, 382C, 382D, 382E, 382F, 382G, 382H, such as bydefining apertures in the thermocouple insertion tube 326 at orproximate the locations 382A, 382B, 382C, 382D, 382E, 382F, 382G, 382Hto allow the temperature measurement device 310 to gauge the temperatureof the reactor interior. While a temperature measurement device has beendescribed, it will be appreciated that the disclosure extends to othertypes of sensors and is not limited to a multi-element thermocouple. Inembodiments, different sensors may be arranged at different locations asnecessary.

The temperature measurement device 310, the reactor 300, and thethermocouple insertion tube 326 advantageously facilitate improvedprocess control by providing granular reactor conditions data atmultiple locations within a reactor while simultaneously minimizing therisk of leakage, particularly for high pressure and/or high temperatureservice and/or for reactions involving hydrogen or catalysts that aresensitive to oxygen, by reducing the number of thermocouple joints. Theconfiguration of the temperature measurement device 310, the reactor300, and the thermocouple insertion tube 326 further improves thescalability of a reactor design, as the arrangement of the thermocoupleinsertion tube 326 and the temperature measurement device 310 allows foran accurate reading of internal reactor conditions regardless of thesize of the reactor, mitigating the difficulty of monitoring reactors inwhich thermowells are arranged radially from a sidewall surface of thereactor and, for larger reactors, disproportionately measure conditionsnear the shell rather than near the center of the reactor.

Additionally, as seen in at least FIGS. 2 and 7 , a reactor may comprisea plurality of temperature measurement devices. The temperaturemeasurement devices may be arranged in any suitable configurationrelative to the reactor shell and to each other. In the embodiment ofFIGS. 2 and 7 , for example, the temperature measurement devices may beoffset from a central longitudinal axis of the reactor by a samedistance and arranged opposite each other. The distance between thetemperature measurement devices may be configured to minimizeinterference with or disturbances in the heat distribution within thereactor, particularly the catalyst bed. The distance may be selected tobe above a minimum threshold at which a hotspot would develop between orproximate the temperature measurement devices due to the resultingdisruption to reactant and product flow and accordingly heatdistribution. Arranging the temperature measurement devices above theminimum threshold thereby avoids performance disruptions of the reactorand improves accuracy of the measurement.

The temperature measurement devices may serve different purposes and/ormay be complementary to each other. In the embodiment of FIGS. 2 and 7 ,the temperature measurement devices are multi-element thermocouples asdescribed regarding FIG. 20 . One of the multi-element thermocouples maybe connected to a process control system, while a second one of themulti-element thermocouples may be connected to a safety instrumentsystem.

Providing a plurality of the multi-element thermocouples advantageouslyconfirms the measurement of temperature at a particular location, i.e.elevation, within the reactor. Any difference between the signalsobtained from the multi-element thermocouples may be used to determine,for example, the development of a hot spot at a particular elevation,allowing an operator to make adjustments as necessary. It will beappreciated that any suitable number of thermocouples in any suitableconfiguration may be used.

An embodiment of the reactor comprises a plurality of feed tubesextending longitudinally through the reactor and a catalyst bed. A tubebundle may define thermocouple insertion tubes extending parallel to thefeed tubes and configured to receive a temperature measurement devicesuch as a multi-element thermocouple therethrough. The thermocoupleinsertion tubes may be configured to extend at different distances froma center of the reactor.

The distances may be configured to allow for measurement of atemperature distribution at different distances from the center. Inparticular, this may help to validate a design of the reactor at aparticular scale, further enhancing the scalability of the reactor ofembodiments of the present disclosure. This further enhances the processcontrol of the reactor, with improved granularity of temperaturemeasurement and the ability to tailor the associated responses using theprocess control system. In embodiments, the radial configuration of thethermocouple insertion tubes may be determined so as to coincide withpredicted hotspots.

This allows an operator to quickly and accurately determine when ahotspot has formed and to respond accordingly, thereby preventingrunaway reactions. The configuration of the thermocouple insertion tubesmay further be determined relative to the tube bundle so as toaccommodate the size of the reactor shell. In smaller reactors, forexample, fewer thermocouple insertion tubes may be utilized, whereas thenumber of thermocouple insertion tubes, and the complexity of theconfiguration of the same, may increase in larger reactors.

FIGS. 21A-21B and FIG. 22 illustrate an alternative reactorconfiguration, although with many similarities to those alreadydescribed herein. As compared to the reactor shown in FIGS. 3-4 , thetop portion of the reactor is modified to reduce the area about whichpotential leaks may occur (e.g., between flanges 112 and 114), toprovide a simplified reactor design, and to reduce cost, For example,the large assembly flange 112, 114 is removed in the embodiment, shownin FIGS. 21A-21B and 22 . Such a separate domed head portion 104 and theassociated flanges are very expensive, heavy, and include a largesurface area for potential leaking points to develop.

In lieu of such a separate domed head portion, reactor 100″ includes adomed head portion 104′ that includes a startup nozzle 110′ including aflange 114 for detachable connection to a reducing flange 112. Startupnozzle 110′ includes a manhole access opening through which amaintenance worker can enter the shell 102 of the reactor, In FIGS.21A-21B and 22 , the domed head portion 104′ is integral with shell 102,without any connecting flanges therebetween. This difference relative tothe reactor 100 provides the described benefits of reduced cost,simplified. design, lighter weight removable top portion, reducedpossibility of leakage, etc.

The manhole access opening through startup nozzle 110′ may be forexample, from 40-80 cm in diameter. Such a manhole access opening may beused to facilitate easier inspection and catalyst loading of thereactor.

As shown in FIGS. 21A-21B and 22 , because of the size of the flange112′, 114′, the thermocouple port 106′ on the domed head portion 104′may be tilted relative to the vertical longitudinal axis 1A. Such aconfiguration still allows measurement of temperatures close to thecenter of reactor 100′. As shown, a reducing flange 112′ is used toconnect startup inlet piping to the manhole access opening, allowingsuch opening to be used as a process connection, as well as for manholeaccess inspection.

As it can be challenging to identify and install the thermocouples, thethermocouple insertion tubes 126 can be configured to extend to agreater height than the other tubes 131. With such a manhole accessopening, this process is simplified, as a worker can access the reactor,load the catalyst, and guide the flexible thermocouples into theappropriate tube. Flexibility of the thermocouples is beneficial, tonavigate the pathway through the tilted thermocouple ports 106′ and theninto the thermocouple insertion tubes 126. Insertion of thethermocouples is far easier where the worker can enter the top of thereactor through the manhole access opening, as compared to thealternative.

By way of example, the tilting of the thermocouple ports 106′ may be atan angle that is from 5° to 30°, or from 10° to 20° (e.g., about 15°)relative to vertical. Of course, other angles may also be possible, suchthat those noted are merely exemplary.

FIG. 23 illustrates a bottom view of the reactor 100′, which is similarto the configuration shown in FIGS. 4 and 5A.

FIGS. 24-31C illustrate other aspects and features that may be includedwithin any of the presently described reactors. For example, slidingstrips 220 are provided around the periphery of the tube bundle 130 andthe tube support plates 162-165. Such sliding strips facilitate easierassembly of the tube bundle and reactor. Such strips 220 also allow forthermal expansion, allowing the strip to slide up and down relative tothe support plates to which it, is slidably attached. For example, asshown in FIGS. 25 and 26 , the top feed tube support plate 150 and eachadditional or intermediate tube support plate 162-165 (plate 162 isshown in FIG. 26 , as exemplary of all intermediate plates 162-165) caninclude one or more peripheral slots 222 a-222 d for receipt of thesliding strip 220. The illustrated configuration includes 4 such slots222 a-222 d, for 4 sliding strips, with two of the slots (222 a and 222b) positioned 30° apart from one another, and the other two slots (222 cand 222 d) also positioned 30° apart from one another, on opposite sidesof the tube bundle and reactor. As shown, slot 222 a is positioned 180°from slot 222 c, and slot 222 b is positioned 180° from slot 222 d. Ofcourse, other configurations including different numbers of slots,sliding strips, and positioning of such slots and sliding strips is alsopossible.

FIG. 27 illustrates a close-up view of a portion of the feed tubesupport plate 162 of FIG. 26 , showing exemplary slot 222 c. FIG. 28illustrates a dose-up of a portion of feed tube support plate 162,illustrating another configuration, similar to that shown in FIG. 8 .

FIG. 29 illustrates a close-up view showing the sliding strip 220 withina slot 222 a, while also showing how each feed tube 131 can include aupper and lower support rings 224 welded or otherwise fixedly attachedto the feed tube 131, both above and below a given feed tube support.plate (e.g., plate 162 is illustrated). The feed tube 131 itself may beslidably disposed relative to plate 162, but attached support rings 224serve as stops, to limit the movement of the tube relative to thesupport plate 162, e.g., so as to accommodate uneven thermal expansion.Each sliding strip 220 is shown as including an opening 226 for receiptof the thickness of the feed tube support plate 162, and a height ofopening 226 is greater than a thickness of plate 162, so as to allowsliding strip 220 to slide up and down according to the dimensions ofsuch opening 226, relative to plate 162, e.g., due to uneven thermalexpansion. Sliding strip 220 is thus not fixedly attached to plate 162(nor are tubes 131 fixedly attached to plate 162), but both the slidingstrip and the tubes are free to slide to some degree relative to plate162, within the bounds set by the stops provided by the support rings224 associated with tubes 131, and the stops provided by the ends ofopenings 226 of sliding strips 220.

FIG. 30 illustrates the sliding strip 220, with its associated openings226, for engagement with each of the various feed tube support plates162-165. As shown, the top of sliding strip 220 also includes an opening228, although this opening is not as large as the other openings 226,but is sized to have a height that is approximately equal to thethickness of the top feed support plate 150, so that the top feedsupport plate 150 is received within slot 228 and fixed relative to thesliding strip, while the openings 226 are sized larger than thethickness of the corresponding received intermediate tube support plates162, 163, 164, and 165, as shown, allowing some degree of play and slidebetween the sliding strip 220 and such intermediate tube support plates162-165. Each of the various sliding strips (e.g., 4 strips) may besimilarly configured. As is apparent from the Figures, the sliding stripmay not extend the full length of the tubes of tube bundle 130, but mayrun from top plate 150 to the lower tube feed support plate 165, with nosubstantial extension of the sliding strip below plate 165, towardscatalyst support plate 154. For example, as shown in FIG. 24 , distance167 between feed tube support plate 165 and the catalyst support plate154, as well as distance 169 between the catalyst support plate 154 andthe gas inlet plate 156 may include no sliding strip.

FIGS. 31A-31C illustrate side or cross-sectional views associated withthe top of the sliding strip 220 (FIG. 31A), the central portion of thesliding strip 220 (FIG. 31B), and the bottom portion of the slidingstrip 220 (FIG. 31C). The configuration shown in FIG. 319 may apply forhowever many intermediate tube support plates are present, below the toptube support plate and the lowest tube support plate (e.g., in theillustrated configuration, this may apply to plates 162, 163, and 164).By way of example, FIG. 31A shows how the top feed support plate 150 maybe fixed relative to sliding strip 220, with the peripheral edge of suchplate 150 engaged within slot 228. FIG. 31B shows how the intermediateplates 162, 163, and 164 engage with sliding strip 220, where theperipheral edge of plate 162 is positioned within opening 226, but theplate 162 and sliding strip 220 are not fixed relative to one another,but strip 220 is free to slide up and down relative to the plate, due tothe sizing of the height of opening 226 relative to the thickness of theplate. FIG. 31C shows the bottom portion of the sliding strip 220, witha similarly sized opening 226 for plate 165, showing how sliding strip220 does not extend significantly downward past plate 165, but ends atplate 165.

By providing a reactor according to the disclosed embodiments, theproblems of existing reactors being difficult to access when maintenanceis needed, and reactors being difficult to scale based on the throughputneeds of a facility, are addressed. The reactor embodiments of thepresent disclosure advantageously provide a reactor that comprisesrobust yet flexible reactor internals that are configured to bemodularly arranged based on the throughput needs of a facility design,easily accessible for maintenance and catalyst loading, facilitateimproved, even distribution of catalyst, reactants, and heat, and/orprovide robust structural support during construction, transportation,installation, and operation.

While the reactor has been illustrated and described in detail in thedrawings and foregoing description, the same is to be considered asillustrative and not restrictive in character, it being understood thatonly the preferred embodiments have been shown and described and thatall changes, equivalents, and modifications that come within the spiritof the embodiments defined by following claims are desired to beprotected.

Accordingly, features of the disclosed embodiments may be combined orarranged for achieving particular advantages as would be understood fromthe disclosure by one of ordinary skill in the art. Similarly, featuresof the disclosed embodiments may provide independent benefits applicableto other examples not detailed herein. In particular, any feature fromone disclosed embodiment may be employed in another disclosedembodiment.

It is to be understood that not necessarily all objects or advantagesmay be achieved under any embodiment of the disclosure. Those skilled inthe art will recognize that the reactor may be embodied or carried outin a manner that achieves or optimizes one advantage or group ofadvantages as taught without achieving other objects or advantages astaught or suggested.

The skilled artisan will recognize the interchangeability of variousdisclosed features. Besides the variations described, other knownequivalents for each feature can be mixed and matched by one of ordinaryskill in this art to make or use a reactor under principles of thepresent disclosure. It will be understood by the skilled artisan thatthe features described may be adapted to other types of reactors,reaction suites, chemical species, and processes. Hence this disclosureand the embodiments and variations thereof are not limited to methanolsynthesis processes or to shell-and-tube reactors, but can be utilizedin any chemical process.

Although this disclosure describes certain exemplary embodiments andexamples of a reactor, it therefore will be understood by those skilledin the art that the present disclosure extends beyond the specificallydisclosed embodiments to other alternative embodiments and/or uses ofthe disclosure and obvious modifications and equivalents thereof. It isintended that the present disclosure should not be limited by theparticular disclosed embodiments described above.

In addition, unless otherwise indicated, numbers expressing quantities,constituents, distances, or other measurements used in the specificationand claims are to be understood as optionally being modified by the term“about” or its synonyms. When the terms “about,” “approximately,”“substantially,” or the like are used in conjunction with a statedamount, value, or condition, it may be taken to mean an amount, value orcondition that deviates by less than 20%, less than 10%, less than 5%,less than 1%, less than 0.1%, or less than 0.01% of the stated amount,value, or condition. As used herein, the term “between” includes anyreferenced endpoints. For example, “between 2 and 10” includes both 2and 10.

1. A reactor comprising: a shell defining an internal space configured to receive a catalyst; a domed head portion that includes a startup nozzle including a flange for detachable connection to a reducing flange, the startup nozzle including a manhole access opening through which a maintenance worker can enter the shell of the reactor; at least one inlet nozzle; and a tube bundle comprising a plurality of tubes arranged in concentric bands about a longitudinal axis of the reactor.
 2. The reactor of claim 1, wherein the domed head portion is integral with the shell, without any connecting flanges therebetween.
 3. The reactor of claim 1, wherein the domed head portion includes at least one thermocouple port, wherein the at least one thermocouple port is at a tilted angle relative to a vertical longitudinal axis of the reactor.
 4. The reactor of claim 3, wherein the domed head portion includes two thermocouple ports, each at a tilted angle relative to the vertical longitudinal axis of the reactor.
 5. The reactor of claim 4, wherein the thermocouple ports are each tilted away from the startup nozzle at an angle of from about 5° to about 30° relative to the vertical longitudinal axis of the reactor.
 6. The reactor of claim 3, wherein a circumferential band of the at least one tube support plate further comprises brackets corresponding to at least one thermocouple insertion tube, wherein the at least one thermocouple insertion tube is configured to receive a temperature measurement device inserted into the reactor through the at least one thermocouple port, the temperature measurement device being configured to obtain a temperature at a plurality of longitudinal locations within the reactor.
 7. The reactor of claim 1, wherein the reactor further comprises at least one tube support plate, wherein the at least one tube support plate comprises at least one circumferential band, wherein the at least one circumferential band comprises at least one bracket configured to extend about a portion of a tube of the tube bundle.
 8. The reactor of claim 7, further comprising at least one of a catalyst support plate, a gas inlet plate, or a top plate.
 9. The reactor of claim 7, wherein the catalyst is a solid catalyst that comprises balls of a first diameter and balls of a second diameter, wherein the reactor further comprises a catalyst support plate, wherein the catalyst balls of the first diameter and the catalyst balls of the second diameter are arranged in discrete, respective layers proximate the catalyst support plate.
 10. The reactor of claim 7, wherein the reactor further comprises a catalyst support plate, wherein the catalyst support plate defines one or more apertures, wherein the one or more apertures comprise a plurality of apertures of a first size and a plurality of apertures of a second size, the apertures extending through at least part of a thickness of the catalyst support plate.
 11. The reactor of claim 10, wherein the first size corresponds to a circumference of at least one tube of the tube bundle, and the second size is smaller than the first size, wherein the apertures of the first size are defined through the catalyst support plate according to an arrangement of the plurality of tubes of the tube bundle.
 12. The reactor of claim 11, wherein the reactor further comprises a gas inlet plate, wherein the gas inlet plate comprises a plurality of apertures defined through a thickness of the gas inlet plate, wherein the plurality of apertures are circular apertures defined through the gas inlet plate according to the arrangement of the plurality of tubes of the tube bundle, wherein the gas inlet plate further comprises a second plurality of apertures defined through the thickness of the gas inlet plate, the second plurality of apertures comprising a different size and/or shape than the plurality of circular apertures.
 13. The reactor of claim 7, wherein the at least one tube support plate defines a plurality of concentric circumferential bands, wherein the at least one tube support plate defines at least one radial strut connected to at least one of the plurality of circumferential bands.
 14. The reactor of claim 1 wherein: the catalyst received within the shell is a solid catalyst, wherein the domed head portion is integral with the shell, without any connecting flanges therebetween; the reactor further comprises an outlet nozzle, the outlet nozzle being located proximate a bottom portion of the shell; the reactor further comprises a catalyst support plate, wherein the outlet nozzle is arranged below the catalyst support plate; the reactor further comprises a plurality of tube support plates, wherein each tube support plate comprises a plurality of circumferential bands, wherein each circumferential band comprises at least one bracket configured to extend about a tube of the tube bundle; wherein each tube support plate defines a plurality of radial struts, each radial strut being connected between the circumferential bands of the tube support plate; wherein each radial strut is removably secured to at least one of the circumferential bands of each tube support plate; and a gas inlet plate, wherein the gas inlet plate is arranged proximate the inlet nozzle, with the inlet nozzle arranged below the gas inlet plate.
 15. A reactor comprising: a shell defining an internal space configured to receive a catalyst; at least one inlet nozzle; and a tube bundle comprising a plurality of tubes arranged in concentric bands about a longitudinal axis of the reactor; wherein the reactor further comprises a catalyst support plate including a plurality of apertures formed therethrough through which the plurality of tubes of the tube bundle pass, wherein a support ring is attached around each tube passing through a corresponding aperture of the catalyst support plate, and wherein the tubes are not fixed relative to the catalyst support plate, to allow for thermal expansion of the tubes passing through the catalyst support plate.
 16. The reactor of claim 15, wherein each tube includes an upper support ring and a lower support ring attached to and extending around each of said tubes, the upper support ring being positioned above the catalyst support plate and the lower support ring being positioned below the catalyst support plate, wherein a spacing between the upper support ring and the lower support ring of a given tube is greater than a thickness of the catalyst support plate.
 17. A reactor comprising: a shell defining an internal space configured to receive a catalyst; at least one inlet nozzle; and a tube bundle comprising a plurality of tubes arranged in concentric bands about a longitudinal axis of the reactor; wherein the reactor further comprises at least one tube support plate, each tube support plate including a plurality of apertures formed therethrough each tube of the plurality of tubes passing through a corresponding aperture of the tube support plate, wherein the reactor further includes at least one sliding strip at a periphery of the at least one tube support plate, wherein at least one of the tube support plates includes at least one slot formed at a periphery of said tube support plate, for receipt of a corresponding sliding strip.
 18. The reactor of claim 17, wherein each sliding strip includes an opening for receipt of a thickness of a corresponding one of the at least one tube support plate, wherein a height of the opening in the sliding strip is greater than a thickness of the corresponding tube support plate.
 19. The reactor of claim 18, wherein the at least one tube support plate includes a top tube support plate and one or more additional tube support plates, wherein the opening of the sliding strip that corresponds to the top tube support plate has a height that is approximately equal to the thickness of the top tube support plate, so that the top tube support plate is fixed relative to the sliding strip, and openings of the sliding strip configured for receipt of the additional tube support plates have heights that are greater than a thickness of their corresponding tube support plates, so that the sliding strip is slidable relative to the additional tube support plates.
 20. The reactor of claim 17, wherein the shell of the reactor further comprises a domed head portion that includes a startup nozzle including a flange for detachable connection to a reducing flange, the startup nozzle including a manhole access opening through which a maintenance worker can enter the shell of the reactor. 